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Reconstruction of past changes in Arctic sea ice extent may be critical for understanding its future evolution. Methanesulfonate (MSA) and bromine concentrations preserved in ice cores have both been proposed as indicators of past sea ice conditions. In this study, two ice cores from central and north-eastern Greenland were analysed at sub-annual resolution for MSA (CH3SO3H) and bromine, covering the time period 1750–2010. We examine correlations between ice core MSA and the HadISST1 ICE sea ice dataset and consult back trajectories to infer the likely source regions. A strong correlation between the low-frequency MSA and bromine records during pre-industrial times indicates that both chemical species are likely linked to processes occurring on or near sea ice in the same source regions. The positive correlation between ice core MSA and bromine persists until the mid-20th century, when the acidity of Greenland ice begins to increase markedly due to increased fossil fuel emissions. After that time, MSA levels decrease as a result of declining sea ice extent but bromine levels increase. We consider several possible explanations and ultimately suggest that increased acidity, specifically nitric acid, of snow on sea ice stimulates the release of reactive Br from sea ice, resulting in increased transport and deposition on the Greenland ice sheet.

Advances in trace gas analysis allow localised, non-atmospheric features to be resolved in ice cores, superimposed on the coherent atmospheric signal. These high-frequency signals could not have survived the low-pass filter effect that gas diffusion in the firn exerts on the atmospheric history and therefore do not result from changes in the atmospheric composition at the ice sheet surface. Using continuous methane (CH4) records obtained from five polar ice cores, we characterise these non-atmospheric signals and explore their origin. Isolated samples, enriched in CH4 in the Tunu13 (Greenland) record are linked to the presence of melt layers. Melting can enrich the methane concentration due to a solubility effect, but we find that an additional in situ process is required to generate the full magnitude of these anomalies. Furthermore, in all the ice cores studied there is evidence of reproducible, decimetre-scale CH4 variability. Through a series of tests, we demonstrate that this is an artifact of layered bubble trapping in a heterogeneous-density firn column; we use the term “trapping signal” for this phenomenon. The peak-to-peak amplitude of the trapping signal is typically 5 ppb, but may exceed 40 ppb. Signal magnitude increases with atmospheric CH4 growth rate and seasonal density contrast, and decreases with accumulation rate. Significant annual periodicity is present in the CH4 variability of two Greenland ice cores, suggesting that layered gas trapping at these sites is controlled by regular, seasonal variations in the physical properties of the firn. Future analytical campaigns should anticipate high-frequency artifacts at high-melt ice core sites or during time periods with high atmospheric CH4 growth rate in order to avoid misinterpretation of such features as past changes in atmospheric composition.

The role of sea ice in the Earth climate system is still under debate, although it is known to influence albedo, ocean circulation, and atmosphere-ocean heat and gas exchange. Here we present a reconstruction of 1950 to 1998 AD sea ice in the Laptev Sea based on the Akademii Nauk ice core (Severnaya Zemlya, Russian Arctic). The chemistry of halogens bromine (Br) and iodine (I) is strongly active and influenced by sea ice dynamics, in terms of physical, chemical and biological process. Bromine reacts on the sea ice surface in autocatalyzing >bromine explosion> events, causing an enrichment of the Br/Na ratio and hence a bromine excess (Br) in snow compared to that in seawater. Iodine is suggested to be emitted from algal communities growing under sea ice. The results suggest a connection between Brexc and spring sea ice area, as well as a connection between iodine concentration and summer sea ice area. The correlation coefficients obtained between Br and spring sea ice (r = 0.44) as well as between iodine and summer sea ice (r = 0.50) for the Laptev Sea suggest that these two halogens could become good candidates for extended reconstructions of past sea ice changes in the Arctic., This study contributes to the Eurasian Arctic Ice 4k project and was supported by the Deutsche Forschungs- gemeinschaft (grant OP 217/2-1 awarded to Thomas Opel). The drilling project on the Akademii Nauk ice cap was funded by the German Ministry of Education and Research (BMBF research project 03PL 027A). Analysis and interpretation of the Akademii Nauk ice core at the Desert Research Institute was funded by US National Science Foundation grant 1023672. The research leading to these results received funding from the European Research Council under the European Community’s Seventh Framework Programme (FP7/2007–2013)/ERC grant agreement no. 610055. We thank the University of Bremen, supported by the State of Bremen; the German Aerospace Center, DLR; and the European Space Agency for the satellite BrO imagines. Opel)

Ice core records from Antarctica show mostly synchronous temperature variations during the last deglacial transition, an indication that the climate of the entire continent reacted as one unit to the global changes. However, a record from the Taylor Dome ice core in the Ross Sea sector of East Antarctica has been suggested to show a rapid warming, similar in style and synchronous with the Oldest Dryas—Bølling warming in Greenland. Since publication of the Taylor Dome record, a number of lines of evidence have suggested that this interpretation is incorrect and reflects errors in the underlying time scale. The issues raised regarding the dating of Taylor Dome currently linger unresolved, and the original time scale remains the de facto chronology. We present new water isotope and chemistry data from nearby Taylor Glacier to resolve the confusion surrounding the Taylor Dome time scale. We find that the Taylor Glacier record is incompatible with the original interpretation of the Taylor Dome ice core, showing that the warming in the area was gradual and started at ∼18 ka BP (before 1950) as seen in other East Antarctic ice cores. We build a consistent, up‐to‐date Taylor Dome chronology from 0 to 60 ka BP by combining new and old age markers based on synchronization to other ice core records. The most notable feature of the new TD2015 time scale is a gas age—ice age difference of up to 12,000 years during the Last Glacial Maximum, by far the largest ever observed.

Knowledge on the occurrence rate of extreme solar storms is strongly limited by the relatively recent advent of satellite monitoring of the Sun. To extend our perspective of solar storms prior to the satellite era and because atmospheric ionization induced by solar energetic particles (SEPs) can lead to the production of odd nitrogen, nitrate spikes in ice cores have been tentatively used to document both the occurrence and intensity of past SEP events. However, the reliability of the use of nitrate in ice records as a proxy for SEP events is strongly debated. This is partly due to equivocal detection of nitrate spikes in single ice cores and possible alternative sources, such as biomass burning plumes. Here we present new continuous high-resolution measurements of nitrate and of the biomass burning species ammonium and black carbon, from several Antarctic and Greenland ice cores. We investigate periods covering the two largest known SEP events of 775 and 994 Common Era as well as the Carrington event and the hard SEP event of February 1956. We report no coincident nitrate spikes associated with any of these benchmark events. We also demonstrate the low reproducibility of the nitrate signal in multiple ice cores and confirm the significant relationship between biomass burning plumes and nitrate spikes in individual ice cores. In the light of these new data, there is no line of evidence that supports the hypothesis that ice cores preserve or document detectable amounts of nitrate produced by SEPs, even for the most extreme events known to date.

International audience; Interpretation of ice core trace gas records depends on an accurate understanding of the processes that smooth the atmospheric signal in the firn. Much work has been done to understand the processes affecting air transport in the open pores of the firn, but a paucity of data from air trapped in bubbles in the firn-ice transition region has limited the ability to constrain the effect of bubble closure processes. Here we present high-resolution measurements of firn density, methane concentrations, nitrogen isotopes, and total air content that show layering in the firn-ice transition region at the West Antarctic Ice Sheet (WAIS) Divide ice core site. Using the notion that bubble trapping is a stochastic process, we derive a new parameterization for closed porosity that incorporates the effects of layering in a steady state firn modeling approach. We include the process of bubble trapping into an open-porosity firn air transport model and obtain a good fit to the firn core data. We find that layering broadens the depth range over which bubbles are trapped, widens the modeled gas age distribution of air in closed bubbles, reduces the mean gas age of air in closed bubbles, and introduces stratigraphic irregularities in the gas age scale that have a peak-to-peak variability of~10 years at WAIS Divide. For a more complete understanding of gas occlusion and its impact on ice core records, we suggest that this experiment be repeated at sites climatically different from WAIS Divide, for example, on the East Antarctic plateau.

Volcanic eruptions contribute to climate variability, but quantifying these contributions has been limited by inconsistencies in the timing of atmospheric volcanic aerosol loading determined from ice cores and subsequent cooling from climate proxies such as tree rings. Here we resolve these inconsistencies and show that large eruptions in the tropics and high latitudes were primary drivers of interannual-to-decadal temperature variability in the Northern Hemisphere during the past 2,500 years. Our results are based on new records of atmospheric aerosol loading developed from high-resolution, multi-parameter measurements from an array of Greenland and Antarctic ice cores as well as distinctive age markers to constrain chronologies. Overall, cooling was proportional to the magnitude of volcanic forcing and persisted for up to ten years after some of the largest eruptive episodes. Our revised timescale more firmly implicates volcanic eruptions as catalysts in the major sixth-century pandemics, famines, and socioeconomic disruptions in Eurasia and Mesoamerica while allowing multi-millennium quantification of climate response to volcanic forcing.

Significance: Cold and dry glacial-state climate conditions persisted in the Southern Hemisphere until approximately 17.7 ka, when paleoclimate records show a largely unexplained sharp, nearly synchronous acceleration in deglaciation. Detailed measurements in Antarctic ice cores document exactly at that time a unique, ∼192-y series of massive halogen-rich volcanic eruptions geochemically attributed to Mount Takahe in West Antarctica. Rather than a coincidence, we postulate that halogen-catalyzed stratospheric ozone depletion over Antarctica triggered large-scale atmospheric circulation and hydroclimate changes similar to the modern Antarctic ozone hole, explaining the synchronicity and abruptness of accelerated Southern Hemisphere deglaciation. Abstract: Glacial-state greenhouse gas concentrations and Southern Hemisphere climate conditions persisted until ∼17.7 ka, when a nearly synchronous acceleration in deglaciation was recorded in paleoclimate proxies in large parts of the Southern Hemisphere, with many changes ascribed to a sudden poleward shift in the Southern Hemisphere westerlies and subsequent climate impacts. We used high-resolution chemical measurements in the West Antarctic Ice Sheet Divide, Byrd, and other ice cores to document a unique, ∼192-y series of halogen-rich volcanic eruptions exactly at the start of accelerated deglaciation, with tephra identifying the nearby Mount Takahe volcano as the source. Extensive fallout from these massive eruptions has been found >2,800 km from Mount Takahe. Sulfur isotope anomalies and marked decreases in ice core bromine consistent with increased surface UV radiation indicate that the eruptions led to stratospheric ozone depletion. Rather than a highly improbable coincidence, circulation and climate changes extending from the Antarctic Peninsula to the subtropics—similar to those associated with modern stratospheric ozone depletion over Antarctica—plausibly link the Mount Takahe eruptions to the onset of accelerated Southern Hemisphere deglaciation ∼17.7 ka.

We present the first long-term, highly resolved prokaryotic cell concentration record obtained from a polar ice core. This record, obtained from the West Antarctic Ice Sheet (WAIS) Divide (WD) ice core, spanned from the Last Glacial Maximum (LGM) to the early Holocene (EH) and showed distinct fluctuations in prokaryotic cell concentration coincident with major climatic states. The time series also revealed a ~1,500-year periodicity with greater amplitude during the Last Deglaciation (LDG). Higher prokaryotic cell concentration and lower variability occurred during the LGM and EH than during the LDG. A sevenfold decrease in prokaryotic cell concentration coincided with the LGM/LDG transition and the global 19 ka meltwater pulse. Statistical models revealed significant relationships between the prokaryotic cell record and tracers of both marine (sea-salt sodium [ssNa]) and burning emissions (black carbon [BC]). Collectively, these models, together with visual observations and methanosulfidic acid (MSA) measurements, indicated that the temporal variability in concentration of airborne prokaryotic cells reflected changes in marine/sea-ice regional environments of the WAIS. Our data revealed that variations in source and transport were the most likely processes producing the significant temporal variations in WD prokaryotic cell concentrations. This record provided strong evidence that airborne prokaryotic cell deposition differed during the LGM, LDG, and EH, and that these changes in cell densities could be explained by different environmental conditions during each of these climatic periods. Our observations provide the first ice-core time series evidence for a prokaryotic response to long-term climatic and environmental processes.

Biomass burning is a major source of greenhouse gases and influences regional to global climate. Pre-industrial fire-history records from black carbon, charcoal and other proxies provide baseline estimates of biomass burning at local to global scales spanning millennia, and are thus useful to examine the role of fire in the carbon cycle and climate system. Here we use the specific biomarker levoglucosan together with black carbon and ammonium concentrations from the North Greenland Eemian (NEEM) ice cores (77.49° N, 51.2° W; 2480 m a.s.l) over the past 2000 years to infer changes in boreal fire activity. Increases in boreal fire activity over the periods 1000–1300 CE and decreases during 700–900 CE coincide with high-latitude NH temperature changes. Levoglucosan concentrations in the NEEM ice cores peak between 1500 and 1700 CE, and most levoglucosan spikes coincide with the most extensive central and northern Asian droughts of the past millennium. Many of these multi-annual droughts are caused by Asian monsoon failures, thus suggesting a connection between low- and high-latitude climate processes. North America is a primary source of biomass burning aerosols due to its relative proximity to the Greenland Ice Cap. During major fire events, however, isotopic analyses of dust, back trajectories and links with levoglucosan peaks and regional drought reconstructions suggest that Siberia is also an important source of pyrogenic aerosols to Greenland.

The sources and transport pathways of aerosol species in Antarctica remain uncertain, partly due to limited seasonally resolved data from the harsh environment. Here, we examine the seasonal cycles of major ions in three high-accumulation West Antarctic ice cores for new information regarding the origin of aerosol species. A new method for continuous acidity measurement in ice cores is exploited to provide a comprehensive, charge-balance approach to assessing the major non-sea-salt (nss) species. The average nss-anion composition is 41% sulfate (SO42−), 36% nitrate (NO3−), 15% excess-chloride (ExCl−), and 8% methanesulfonic acid (MSA). Approximately 2% of the acid-anion content is neutralized by ammonium (NH4+), and the remainder is balanced by the acidity (Acy ≈ H+ − HCO3−). The annual cycle of NO3− shows a primary peak in summer and a secondary peak in late winter/spring that are consistent with previous air and snow studies in Antarctica. The origin of these peaks remains uncertain, however, and is an area of active research. A high correlation between NH4+ and black carbon (BC) suggests that a major source of NH4+ is midlatitude biomass burning rather than marine biomass decay, as previously assumed. The annual peak in excess chloride (ExCl−) coincides with the late-winter maximum in sea ice extent. Wintertime ExCl− is correlated with offshore sea ice concentrations and inversely correlated with temperature from nearby Byrd station. These observations suggest that the winter peak in ExCl− is an expression of fractionated sea-salt aerosol and that sea ice is therefore a major source of sea-salt aerosol in the region.

Assessments of climate sensitivity to projected greenhouse gas concentrations underpin environmental policy decisions, with such assessments often based on model simulations of climate during recent centuries and millennia1, 2, 3. These simulations depend critically on accurate records of past aerosol forcing from global-scale volcanic eruptions, reconstructed from measurements of sulphate deposition in ice cores4, 5, 6. Non-uniform transport and deposition of volcanic fallout mean that multiple records from a wide array of ice cores must be combined to create accurate reconstructions. Here we re-evaluated the record of volcanic sulphate deposition using a much more extensive array of Antarctic ice cores. In our new reconstruction, many additional records have been added and dating of previously published records corrected through precise synchronization to the annually dated West Antarctic Ice Sheet Divide ice core7, improving and extending the record throughout the Common Era. Whereas agreement with existing reconstructions is excellent after 1500, we found a substantially different history of volcanic aerosol deposition before 1500; for example, global aerosol forcing values from some of the largest eruptions (for example, 1257 and 1458) previously were overestimated by 20–30% and others underestimated by 20–50%.

We present a detailed comparison between subsequent versions of commercially available wavelength-scanned cavity ring-down water isotope analysers (L2120-i and L2130-i, Picarro Inc.). The analysers are used in parallel in a continuous mode by adaption of a low-volume flash evaporation module. Application of the analysers to ice-core analysis is assessed by comparison between continuous water isotope measurements of a glacial ice-core from Severnaya Zemlya with discrete isotope-ratio mass spectrometry measurements performed on parallel samples from the same ice-core. The great advances between instrument versions, particularly in the measurement of δ(2)H, allow the continuous technique to achieve the same high level of accuracy and precision obtained using traditional isotope spectrometry techniques in a fraction of the experiment time. However, when applied to continuous ice-core measurements, increased integration times result in a compromise of the achievable depth resolution of the ice-core records.

The cause of warming in the Southern Hemisphere during the most recent deglaciation remains a matter of debate. Hypotheses for a Northern Hemisphere trigger, through oceanic redistributions of heat, are based in part on the abrupt onset of warming seen in East Antarctic ice cores and dated to 18,000 years ago, which is several thousand years after high-latitude Northern Hemisphere summer insolation intensity began increasing from its minimum, approximately 24,000 years ago. An alternative explanation is that local solar insolation changes cause the Southern Hemisphere to warm independently. Here we present results from a new, annually resolved ice-core record from West Antarctica that reconciles these two views. The records show that 18,000 years ago snow accumulation in West Antarctica began increasing, coincident with increasing carbon dioxide concentrations, warming in East Antarctica and cooling in the Northern Hemisphere associated with an abrupt decrease in Atlantic meridional overturning circulation. However, significant warming in West Antarctica began at least 2,000 years earlier. Circum-Antarctic sea-ice decline, driven by increasing local insolation, is the likely cause of this warming. The marine-influenced West Antarctic records suggest a more active role for the Southern Ocean in the onset of deglaciation than is inferred from ice cores in the East Antarctic interior, which are largely isolated from sea-ice changes.

Volcanism is a natural climate forcing causing short-term variations in temperatures. Histories of volcanic eruptions are needed to quantify their role in climate variability and assess human impacts. We present two new seasonally resolved, annually dated non-sea-salt sulfur records from polar ice cores - WAIS Divide (WDC06A) from West Antarctica spanning 408 B.C.E. to 2003 C.E. and NEEM (NEEM-2011-S1) from Greenland spanning 78 to 1997 C.E. - both analyzed using high-resolution continuous flow analysis coupled to two mass spectrometers. The high dating accuracy allowed placing the large bi-hemispheric deposition event ascribed to the eruption of Kuwae in Vanuatu (previously thought to be 1452/1453 C.E. and used as a tie-point in ice core dating) into the year 1458/1459 C.E. This new age is consistent with an independent ice core timescale from Law Dome and explains an apparent delayed response in tree rings to this volcanic event. A second volcanic event is detected in 1453 C.E. in both ice cores. We show for the first time ice core signals in Greenland and Antarctica from the strong eruption of Taupo in New Zealand in 232 C.E. In total, 133 volcanic events were extracted from WDC06A and 138 from NEEM-2011-S1, with 50 ice core signals - predominantly from tropical source volcanoes - identified simultaneously in both records. We assess the effect of large bipolar events on temperature-sensitive tree ring proxies. These two new volcanic records, synchronized with available ice core records to account for spatial variability in sulfate deposition, provide a basis for improving existing time series of volcanic forcing.

International audience; We present the WD2014 chronology for the upper part (0–2850 m; 31.2 ka BP) of the West Antarctic Ice Sheet (WAIS) Divide (WD) ice core. The chronology is based on counting of annual layers observed in the chemical, dust and electrical conductivity records. These layers are caused by seasonal changes in the source, transport, and deposi-tion of aerosols. The measurements were interpreted manually and with the aid of two automated methods. We validated the chronology by comparing to two high-accuracy, absolutely dated chronologies. For the Holocene, the cos-mogenic isotope records of 10 Be from WAIS Divide and 14 C for IntCal13 demonstrated that WD2014 was consistently accurate to better than 0.5 % of the age. For the glacial period, comparisons to the Hulu Cave chronology demonstrated that WD2014 had an accuracy of better than 1 % of the age at three abrupt climate change events between 27 and 31 ka. WD2014 has consistently younger ages than Green-land ice core chronologies during most of the Holocene. For Published by Copernicus Publications on behalf of the European Geosciences Union. 770 M. Sigl et al.: The WAIS Divide deep ice core WD2014 chronology the Younger Dryas–Preboreal transition (11.595 ka; 24 years younger) and the Bølling–Allerød Warming (14.621 ka; 7 years younger), WD2014 ages are within the combined uncertainties of the timescales. Given its high accuracy, WD2014 can become a reference chronology for the Southern Hemisphere, with synchronization to other chronologies feasible using high-quality proxies of volcanism, solar activity , atmospheric mineral dust, and atmospheric methane concentrations.

We explore the collisional energy transfer dynamics of benzene molecules spontaneously evaporating from an in vacuo water–ethanol liquid beam. We find that rotations are cooled significantly more than the lowest-energy vibrational modes, while the rotational energy distributions are Boltzmann. Within experimental uncertainty, the rotational temperatures of vibrationally-excited evaporating molecules are the same as the ground state. Collision-induced gas phase energy transfer measurements reveal that benzene undergoes fast rotational relaxation, from which we deduce that the rotational temperature measured in the evaporation experiments (200–230 K) is an indication of the translational energy of the evaporate. Conversely, vibrational relaxation of the high frequency mode, ν6, is very inefficient, suggesting that the ν6 temperature (260–270 K) is an indication of the liquid surface temperature. Modelling of the relaxation dynamics by both ‘temperature gap’ and ‘Master Equation’ approaches indicates that the equivalent of 150–260 hard-sphere collisions occur during the transition from liquid to vacuum.

We use the liquid microjet technique coupled with laser spectroscopy to measure the rotational and vibrational energy content of benzene spontaneously evaporating from a water−ethanol solution. We ...

The causal mechanisms responsible for the abrupt climate changes of the Last Glacial Period remain unclear. One major difficulty is dating ice-rafted debris deposits associated with Heinrich events: Extensive iceberg influxes into the North Atlantic Ocean linked to global impacts on climate and biogeochemistry. In a new ice core record of atmospheric methane with ultrahigh temporal resolution, we find abrupt methane increases within Heinrich stadials 1, 2, 4, and 5 that, uniquely, have no counterparts in Greenland temperature proxies. Using a heuristic model of tropical rainfall distribution, we propose that Hudson Strait Heinrich events caused rainfall intensification over Southern Hemisphere land areas, thereby producing excess methane in tropical wetlands. Our findings suggest that the climatic impacts of Heinrich events persisted for 740 to 1520 years.

The tropical impact of iceberg armadas The massive discharges of icebergs from the Greenland ice sheet during the Last Glacial Period are called Heinrich events. But did Heinrich events cause abrupt climate change, or were they a product of it? Methane levels represent a proxy for climate, because methane production increases mostly due to wetter conditions in the tropics. Rhodes et al. report a highly resolved record of atmospheric methane concentrations, derived from an ice core from Antarctica. Methane levels varied—i.e., the tropical climate changed—in response to cooling in the Northern Hemisphere caused by Heinrich events. Science , this issue p. 1016

The last glacial period exhibited abrupt Dansgaard-Oeschger climatic oscillations, evidence of which is preserved in a variety of Northern Hemisphere palaeoclimate archives. Ice cores show that Antarctica cooled during the warm phases of the Greenland Dansgaard-Oeschger cycle and vice versa, suggesting an interhemispheric redistribution of heat through a mechanism called the bipolar seesaw. Variations in the Atlantic meridional overturning circulation (AMOC) strength are thought to have been important, but much uncertainty remains regarding the dynamics and trigger of these abrupt events. Key information is contained in the relative phasing of hemispheric climate variations, yet the large, poorly constrained difference between gas age and ice age and the relatively low resolution of methane records from Antarctic ice cores have so far precluded methane-based synchronization at the required sub-centennial precision. Here we use a recently drilled high-accumulation Antarctic ice core to show that, on average, abrupt Greenland warming leads the corresponding Antarctic cooling onset by 218 ± 92 years (2σ) for Dansgaard-Oeschger events, including the Bølling event; Greenland cooling leads the corresponding onset of Antarctic warming by 208 ± 96 years. Our results demonstrate a north-to-south directionality of the abrupt climatic signal, which is propagated to the Southern Hemisphere high latitudes by oceanic rather than atmospheric processes. The similar interpolar phasing of warming and cooling transitions suggests that the transfer time of the climatic signal is independent of the AMOC background state. Our findings confirm a central role for ocean circulation in the bipolar seesaw and provide clear criteria for assessing hypotheses and model simulations of Dansgaard-Oeschger dynamics.

Interior Antarctica is among the most remote places on Earth and was thought to be beyond the reach of human impacts when Amundsen and Scott raced to the South Pole in 1911. Here we show detailed measurements from an extensive array of 16 ice cores quantifying substantial toxic heavy metal lead pollution at South Pole and throughout Antarctica by 1889 - beating polar explorers by more than 22 years. Unlike the Arctic where lead pollution peaked in the 1970s, lead pollution in Antarctica was as high in the early 20 th century as at any time since industrialization. The similar timing and magnitude of changes in lead deposition across Antarctica, as well as the characteristic isotopic signature of Broken Hill lead found throughout the continent, suggest that this single emission source in southern Australia was responsible for the introduction of lead pollution into Antarctica at the end of the 19 th century and remains a significant source today. An estimated 660 €...t of industrial lead have been deposited over Antarctica during the past 130 years as a result of mid-latitude industrial emissions, with regional-to-global scale circulation likely modulating aerosol concentrations. Despite abatement efforts, significant lead pollution in Antarctica persists into the 21 st century.

Biomass burning is a major source of greenhouse gases and influences regional to global climate. Pre-industrial fire-history records from black carbon, charcoal and other proxies provide baseline estimates of biomass burning at local to global scales, but there remains a need for broad-scale fire proxies that span millennia in order to understand the role of fire in the carbon cycle and climate system. We use the specific biomarker levoglucosan, and multi-source black carbon and ammonium concentrations to reconstruct fire activity from the North Greenland Eemian (NEEM) ice cores (77.49° N; 51.2° W, 2480 m a.s.l.) over the past 2000 years. Increases in boreal fire activity (1000–1300 CE and 1500–1700 CE) over multi-decadal timescales coincide with the most extensive central and northern Asian droughts of the past two millennia. The NEEM biomass burning tracers coincide with temperature changes throughout much of the past 2000 years except for during the extreme droughts, when precipitation changes are the dominant factor. Many of these multi-annual droughts are caused by monsoon failures, thus suggesting a connection between low and high latitude climate processes. North America is a primary source of biomass burning aerosols due to its relative proximity to the NEEM camp. During major fire events, however, isotopic analyses of dust, back-trajectories and links with levoglucosan peaks and regional drought reconstructions suggest that Siberia is also an important source of pyrogenic aerosols to Greenland.

Benzene molecules were desorbed from an in vacuo aqueous liquid beam by direct irradiation of the beam with an IR laser tuned to the 2.85 μm absorption band of water. Spectroscopic interrogation of the desorbed benzene molecules was performed via 1 + 1 Resonance-Enhanced Multi-photon Ionisation (REMPI). Rotational contour analyses of the 610 vibronic transition of benzene were performed to determine the rotational temperature of those molecules ejected during the desorption event. At the peak of the desorption plume density, the rotational temperatures were found to be up to ∼100 K lower than that recorded for molecules spontaneously evaporating from the liquid surface. At longer IR-UV laser delay times the benzene rotational temperatures are found to return to those observed following spontaneous evaporation. No evidence of IR desorbed neutral or cationic benzene-containing clusters was observed. However, ionic clusters were observed to be formed after REMPI of the benzene monomer. Analysis of the benzene intensity and that of post-REMPI formed clusters as a function of IR-UV delay shows that number density and local translational temperature vary along the desorption plume.

Here, we review different attempts made since the early 1990s to reconstruct past forest fire activity using chemical signals recorded in ice cores extracted from the Greenland ice sheet and a few mid-northern latitude, high-elevation glaciers. We first examined the quality of various inorganic (ammonium, nitrate, potassium) and organic (black carbon, various organic carbon compounds including levoglucosan and numerous carboxylic acids) species proposed as fire proxies in ice, particularly in Greenland. We discuss limitations in their use during recent vs. pre-industrial times, atmospheric lifetimes, and the relative importance of other non-biomass-burning sources. Different high-resolution records from several Greenland drill sites and covering various timescales, including the last century and Holocene, are discussed. We explore the extent to which atmospheric transport can modulate the record of boreal fires from Canada as recorded in Greenland ice. Ammonium, organic fractions (black and organic carbon), and specific organic compounds such as formate and vanillic acid are found to be good proxies for tracing past boreal fires in Greenland ice. We show that use of other species – potassium, nitrate, and carboxylates (except formate) – is complicated by either post-depositional effects or existence of large non-biomass-burning sources. The quality of levoglucosan with respect to other proxies is not addressed here because of a lack of high-resolution profiles for this species, preventing a fair comparison. Several Greenland ice records of ammonium consistently indicate changing fire activity in Canada in response to past climatic conditions that occurred during the last millennium and since the last large climatic transition. Based on this review, we make recommendations for further study to increase reliability of the reconstructed history of forest fires occurring in a given region.